Ab initio study of magnetism in pristine and defective MnBi2Te4

The magnetic material MnBi2Te4 (MBT) has garnered significant attention due to its unique combination of long-range antiferromagnetism and nontrivial topological electronic properties. However, experimental measurements report inconsistent magnetizations, which could be attributed to a variety of intrinsic defects. To date, a comprehensive investigation of defect-engineered MBT systems has not yet been established. Employing state-of-the-art $ab~initio$ techniques, this work systematically investigates the influence of various experimentally reported defects on the magnetic properties of bulk and monolayer MBT at different concentrations. Mn-vacancy and Mn-rich defects are found to enhance the ferromagnetism of bulk MBT. The investigation of Mn-rich and intermixing defects in the monolayer reveals that subtle structural and electronic modifications can alter the magnetic coupling. Projection onto a Heisenberg Hamiltonian demonstrates that defects modify exchange interactions, thereby giving rise to distinct magnetic ground states. This work sheds light on magnetic coupling mechanisms and provides guidelines for the experimental control of magnetism in MnBi2Te4.